Tailored Porous Electrode Resistance for Controlling Electrolyte Depletion and Improving Charging Response in Electrochemical Systems

Abstract: The rapid charging and/or discharging of electrochemical cells can lead to localized depletion of electrolyte concentration. This depletion can significantly impact the system's time dependent resistance. For systems with porous electrodes, electrolyte depletion can limit the rate of charging and increase energy dissipation. Here we propose a theory to control and avoid electrolyte depletion by tailoring the value and spatial distribution of resistance in a porous electrode. We explore the somewhat counterintuitive idea that increasing local spatial resistances of the solid electrode itself leads to improved charging rate and minimal change in energy loss. We analytically derive a simple expression for an electrode resistance profile that leads to highly uniform electrolyte depletion. We use numerical simulations to explore this theory and simulate spatiotemporal dynamics of electrolyte concentration in the case of a supercapacitor with various tailored electrode resistance profiles which avoid localized depletion. This increases charging rate up to around 2-fold with minimal effect on overall dissipated energy in the system.